Abstract
Abstract The second-order molecular hyperpolarizabilities of 4-aminostilbene, p-nitroaniline and 2-methyl-4-nitroaniline were calculated using photophysical parameters obtained by electronic spectra measurements and the effects of solvents on the spectra. The lowest energy absorption band of the molecules was found to be composed of two transitions, indicating that the well-known two-level model does not apply well to these molecules. The three-level model was developed to evaluate the second-order molecular hyperpolarizability for systems having low energy double transitions. In it the second excited state is explicitly taken into account in the calculation, in addition to the first excited and ground state. The second-order molecular hyperpolarizabilities calculated using the three-level model gave excellent agreement with the observed values determined by the dcSHG technique.
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